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Solvent-free hydrogenation of levulinic acid to γ-valerolactone using a Shvo catalyst precursor: optimization, thermodynamic insights, and life cycle assessment

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Abstract

The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) using the η4-(2,3,4,5-tetraphenylcyclopentadienone) ruthenium tricarbonyl precursor of the well-known Shvo catalyst and H2 pressure was established under solvent-free conditions to achieve 100% conversion and 100% selectivity within 5 hours. Kinetic reaction curves were measured in order to deduce the optimal reaction conditions, which were further evaluated by means of density functional theory (DFT) calculations, and compared with catalytic concepts that consume formic acid or isopropyl alcohol as hydrogen donor. Ultimately, this alternative reaction procedure was subjected to a life cycle assessment (LCA) in comparison with the transfer hydrogenation methodologies, in order to verify its contribution towards a practice of environmentally benign chemistry.

Graphical abstract: Solvent-free hydrogenation of levulinic acid to γ-valerolactone using a Shvo catalyst precursor: optimization, thermodynamic insights, and life cycle assessment

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Article information


Submitted
21 Jun 2019
Accepted
09 Dec 2019
First published
08 Jan 2020

This article is Open Access

Green Chem., 2020, Advance Article
Article type
Paper

Solvent-free hydrogenation of levulinic acid to γ-valerolactone using a Shvo catalyst precursor: optimization, thermodynamic insights, and life cycle assessment

C. A. M. R. van Slagmaat, M. A. F. Delgove, J. Stouten, L. Morick, Y. van der Meer, K. V. Bernaerts and S. M. A. De Wildeman, Green Chem., 2020, Advance Article , DOI: 10.1039/C9GC02088H

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